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Low-temperature catalytic hydrogenation of bio-based furfural and relevant aldehydes using cesium carbonate and hydrosiloxane

机译:使用碳酸铯和氢硅氧烷的生物基糠醛和相关醛的低温催化氢化

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摘要

Selective hydrogenation of unsaturated compounds is mainly carried out by using high-pressure hydrogen in the presence of a precious or transition metal catalyst. Here, we describe a benign approach to efficiently catalyze the hydrogenation of furfural (FUR) to furfuryl alcohol (FFA) over commercially available cesium carbonate using nontoxic and cheap polymethylhydrosiloxane (PMHS) as hydrogen source. Good to excellent FFA yields (= 90%) could be obtained at 25-80 degrees C by appropriate control of the catalyst dosage, reaction time, and the hydride amount. FUR-to-FFA hydrogenation was clarified to follow a pseudo-first order kinetics with low apparent activation energy of 20.6 kJ mol(-1). Mechanistic insights manifested that PMHS was redistributed to H3SiMe, which acted as the active silane for the hydrogenation reactions. Importantly, this catalytic system was able to selectively reduce a wide range of aromatic aldehydes to the corresponding alcohols in good yields of 81-99% at 25-80 degrees C in 2-6 h.
机译:不饱和化合物的选择性氢化主要通过在贵金属或过渡金属催化剂存在下使用高压氢来进行。在这里,我们描述了一种良性方法,以利用无毒和廉价的聚甲基氢硅氧烷(PMH)作为氢气来源,有效地将糠醛(FFA)氢化成糠醇(FFA)氢化成糠醇(FFA)。通过适当控制催化剂剂量,反应时间和氢化物量,可以在25-80℃下获得优异的FFA产量(& = 90%)。澄清了Fur-to-FFA氢化以遵循伪第一阶动力学,低表观活化能量为20.6kJ摩尔(-1)。机械洞察力表现出PMH被重新分配到H3SIME,其作为氢化反应的活性硅烷作用。重要的是,这种催化系统能够在2-6小时内以81-80℃的良好产量为81-99%的产量选择性地减少各种芳香族醛。

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  • 来源
    《RSC Advances》 |2019年第6期|共9页
  • 作者单位

    Guizhou Univ State Key Lab Breeding Base Green Pesticide &

    Agr State Local Joint Lab Comprehens Utilizat Biomass Key Lab Green Pesticide &

    Agr Bioengn Minst Educ Guiyang 550025 Guizhou Peoples R China;

    Guizhou Univ State Key Lab Breeding Base Green Pesticide &

    Agr State Local Joint Lab Comprehens Utilizat Biomass Key Lab Green Pesticide &

    Agr Bioengn Minst Educ Guiyang 550025 Guizhou Peoples R China;

    Guizhou Univ State Key Lab Breeding Base Green Pesticide &

    Agr State Local Joint Lab Comprehens Utilizat Biomass Key Lab Green Pesticide &

    Agr Bioengn Minst Educ Guiyang 550025 Guizhou Peoples R China;

    Guizhou Univ State Key Lab Breeding Base Green Pesticide &

    Agr State Local Joint Lab Comprehens Utilizat Biomass Key Lab Green Pesticide &

    Agr Bioengn Minst Educ Guiyang 550025 Guizhou Peoples R China;

    Guizhou Univ State Key Lab Breeding Base Green Pesticide &

    Agr State Local Joint Lab Comprehens Utilizat Biomass Key Lab Green Pesticide &

    Agr Bioengn Minst Educ Guiyang 550025 Guizhou Peoples R China;

    Guizhou Univ State Key Lab Breeding Base Green Pesticide &

    Agr State Local Joint Lab Comprehens Utilizat Biomass Key Lab Green Pesticide &

    Agr Bioengn Minst Educ Guiyang 550025 Guizhou Peoples R China;

    Guizhou Univ State Key Lab Breeding Base Green Pesticide &

    Agr State Local Joint Lab Comprehens Utilizat Biomass Key Lab Green Pesticide &

    Agr Bioengn Minst Educ Guiyang 550025 Guizhou Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
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